Chemosphere 279 (2021) 130473

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Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

Recent advances in development of nanostructured photodetectors

from ultraviolet to infrared region: A review
P.V. Karthik Yadav a, B. Ajitha b, Y. Ashok Kumar Reddy a, *, Adem Sreedhar c, **
a
Department of Physics, Indian Institute of Information Technology, Design and Manufacturing, Kancheepuram, Off Vandalur-Kelambakkam Road, Chennai,
600127, India
b
Division of Physics, School of Advanced Sciences, Vellore Institute of Technology (VIT), Vandalur - Kelambakkam Road, Chennai, 600127, India
c
Department of Physics, Gachon University, 1342 Seongnamdaero, Sujeong-gu, Seongnam-si, Gyeonggi-do, 461701, Republic of Korea

h i g h l i g h t s g r a p h i c a l a b s t r a c t

Systematically classified the photo-

detector materials based upon their
spectral absorbance.

Basic mechanism and prominent fig-
ures of merit of photodetectors are
explained.

The dependence of PD performance
on various nanostructures are
discussed.

Most recent advancements in photo-
detectors are addressed by expound
of their problems.

a r t i c l e i n f o a b s t r a c t

Article history: Herein, we aim to evaluate the photodetector performance of various nanostructured materials (thin
Received 18 January 2021 films, 2-D nanolayers, 1-D nanowires, and 0-D quantum dots) in ultraviolet (UV), visible, and infrared (IR)
Received in revised form regions. Specifically, semiconductor-based metal oxides such as ZnO, Ga2O3, SnO2, TiO2, and WO3 are the
10 March 2021
majority preferred materials for UV photodetection due to their broad band gap, stability, and relatively
Accepted 30 March 2021
Available online 12 April 2021
simple fabrication processes. Whereas, the graphene-based hetero- and nano-structured composites are
considered as prominent visible light active photodetectors. Interestingly, graphene exhibits broad band
Handling Editor: Derek Muir spectral absorption and ultra-high mobility, which derives graphene as a suitable candidate for visible
detector. Further, due to the very low absorption rate of graphene (2%), various materials have been
Keywords: integrated with graphene (rGO-CZS, PQD-rGO, N-SLG, and GO doped PbI2). In the case of IR photode-
Photodetector tectors, quantum dot IR detectors prevails significant advantage over the quantum well IR detectors due
Ultra-violet to the 0-D quantum confinement and ability to absorb the light with any polarization. In such a way, we
Visible discussed the most recent developments on IR detectors using InAs and PbS quantum dot nano-
Infrared
structures. Overall, this review gives clear view on the development of suitable device architecture under
Nanostructure
prominent nanostructures to tune the photodetector performance from UV to IR spectral regions for
wide-band photodetectors.
© 2021 Elsevier Ltd. All rights reserved.

1. Introduction
* Corresponding author.
** Co-corresponding author.
In the past two decades, we have witnessed tremendous
E-mail addresses: akreddy111@gmail.com (Y.A. Kumar Reddy), ademsvu@gmail.
com (A. Sreedhar). development in material science and nanotechnology, which has

https://doi.org/10.1016/j.chemosphere.2021.130473
0045-6535/© 2021 Elsevier Ltd. All rights reserved.
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

been leading to strengthening of nanoelectronics technology

(Khomutov et al., 2003). Specifically, various novel composite ma-
terials have been replaced traditional materials due to their drastic
effect on our environment and poor device performance. In this
viewpoint, researchers have been adopted various experimental
techniques to constitute the novel materials under essential
nanoscale structures, including nanowires, quantum dots, nano-
belts, and thin films (Wang et al., 2020a; Ponraj et al., 2016). For
this, strategic of fabrication methods including magnetron sput-
tering, electron beam evaporation, chemical vapor deposition
(CVD), electrochemical and mechanical exfoliation, chemical
etching, pulsed laser deposition (PLD), and spray pyrolysis have
been paid great attention due to the potential high surface to vol-
ume ratio and stability with fewer defects (Zeng et al., 2012; Xia
et al., 1999; Liu et al., 2005).
Because of the enriched physical and chemical properties, the
nanostructures have emerged as attractive materials in the field of
nanoelectronics, energy, optoelectronics, photocatalysis, sensors,
drug delivery, biomedicine, lasers, and flexible technology (Wang,
2007; Laurenti et al., 2019; Cheng et al., 2017). In this era of
modernization, most of the electronic devices directly or indirectly
associated with the light interaction in various applications. For
example, many diseases have been treated under powerful light
exposures (lasers). In this point of view, photodetectors (PDs) have
attracted considerable attention, which can effectively detect and
measure the incident light. Specifically, photodetector technology
practically applied in (i) ultra-violet (UV) region for ozone sensing,
pollution detection, gas sensors, and flame detection, (ii) visible
(Vis) region for energy, fiberoptic communications, video imaging,
and artificial vision, and (iii) infrared (IR) region for bio-medical
imaging, defence, space telescopes, and meteorology.
It is well-known that wide range of materials has been used for
the PDs application including metal oxides, transition metal halides
and perovskites. It is to be highlighted that if the composite ma-
terials integrated with different nanostructures, the sensitivity of
the device can be greatly improved. Therefore, it is necessary to
develop and explore the suitability of selective material for
improved photodetector performance. In recent years, nanosheets
of WO3 PD are sensitive to UV light (365 nm) with responsivity of
293 A/W (Liu et al., 2015). On the other hand, WO3 nanowires
showed sensitive to visible light (404 nm) and produced the
responsivity about 19 A/W (Wang et al., 2020b). Therefore, the
reliability of PDs performance depends on key aspects, which
including band gap, crystallinity, and particle size. In addition, thin
Fig. 1. Schematic outline of (a) applications and (b) review presentation on UV, visible,
film PDs have also been developed under good responsivity, which and IR photodetectors.
can be easily scalable for mass production. However, their response
time is lagging due to the poor charge carrier mobility. Moreover,
flexible PDs technology is emerging in smart phones, wearable renders its applicability in various fields. Therefore, we divided the
technology, smart watches, and electronic tattoos. For this, ultra- review paper into three major sections, which bring the simplicity
thin materials are necessary with high efficiency (De Fazio et al., of UV, visible, and IR photodetectors performance. Specifically, we
2016). Typically, nanostructured materials are favored for the have highlighted modern advancements on photodetector tech-
development of photodetector technology due to their attractive nology (UV, Vis, and IR regions) by considering the progressive
electronic properties, photo sensitivity, high charge carrier categorization of material composition under spectral selectivity.
mobility, and flexible nature (Zhang et al., 2020). Therefore, various The overall gist of the present review is illustrated in the Fig. 1(b). In
PDs based on vivid nanostructures (nanowires, nanorods, and particular, we tried to reveal the spectral absorption based on the
quantum dots) have been developed as IR photodetectors to device architecture such as thin films, nanosheets, nanowires,
enhance the response speed and as well as to achieve superior nanocrystals, and quantum dots towards superior photodetector
figure of merits. Hence, this review summarizes the accomplish- performance.
ments of current PDs technology based on different nanostructures
and also provides constructive discussion and challenges faced. 1.1. Photodetector mechanism
Based on the above spectral detectivity, photodetectors have
been classified into three major categories (UV, Vis, and IR photo- Photodetectors emerged as a sensor of incident light, which
detectors) (Zhai et al., 2009). In recent years, concise applicability of mainly used to convert the incident photon energy into electrical
emerging UV, Vis and IR photodetectors in various fields system- signal. Typically, the sensing capacity of incident radiation can be
atically represented in Fig. 1(a). Thus, photodetector performance greatly estimated by measuring the current or voltage signal
2
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

generated in the device. Thus, there is immense interest on the field results in short-circuit current (Isc) during closed circuit. On
development of various photodetectors. Until now, many re- the other hand, separation of opposite charge carriers on either side
searchers reported various photodetector mechanisms enabled in allows for successful photovoltage (Voc) generation.
the UV, Vis and IR regions. Therefore, it is necessary to develop the
strategic device architecture under various composite materials to
improve the sensing of incident light. In such a way, achieving 1.2. Prominent figures of merit
superior photoresponsivity and photodetector sensing mechanism
primarily related to the photoconductive, photogating, and It is well known that prominent features for superior photode-
photovoltaic effects. tector performance are responsivity, detectivity, noise equivalent
power, and external quantum efficiency. This means that the
1.1.1. Photoconductive effect importance of figures of merit can be illustrated irrespective of film
Photoconduction process is one of the important features to thickness, active area of the material, mechanism, architecture, and
develop the high-performance photoconductors. Generally, the working conditions.
structure of photoconductor contains two metal-electrode contacts In order to quantify the photocurrent generation per unit of
at both ends of the semiconductor, which establishes the ohmic- illuminating radiation, responsivity of the photodetector is the key
contact between semiconductor and metal-electrode. Thus, this parameter. The photoresponsivity (Rl) is the ratio between photo-
device architecture illustrates the advantage of photoconduction current generation and incident light energy. The following
mechanism by absorbing the incident light. As a result, electron- expression ensures the responsivity of the photodetector (Omnes
hole pair generation and separation can be effectively facilitated et al., 2007),
under electrons transfer from semiconductor to one end of elec-
trode and holes to another end of electrode. However, superior Iph
photocurrent generation and separation of charge carriers are Rl ¼ (1)
Pin A
directly proportional to the applied potential. Moreover, photo-
current generation also depend on the charge carrier mobility and where, Iph, Pin, and A are photocurrent generation, power density of
lifetime of the developed semiconductor. It should be noted that incident light, and effective area of the photo-active material,
the photoconduction mechanism is predominantly seen in metal- respectively.
semiconductor-metal (M-S-M) structured PDs. The M-S-M PDs To explain the minimum amount of illumination power required
consists of a simple planar structure with interdigited electrodes, to produce a signal to noise ratio (SNR) of 1 at 1 Hz of bandwidth,
which can be easily integrated with other components in the op- noise equivalent power (NEP) is the perfect tool. The following
toelectronic circuits. In addition to that, M-S-M PDs provide less equation represents NEP of the photodetector (Omnes et al., 2007),
transit times for photogenerated charge carriers and possess high
sensitivity. Accordingly, development of strategic approaches is in
necessary to develop the metal-semiconductor-metal (M-S-M) NEP ¼ (2)
Rl
based PDs.
where, in is the noise current and Rl is the responsivity. It should be
1.1.2. Photogating effect highlighted that better photodetector performance can be achieved
Furthermore, photogating effect is also a unique case of photo- at reduced NEP value. According to the equation (2), NEP is directly
conductive effect. Previous reports presented two kinds of photo- proportional to the noise current, which is mainly associated with
gating effect on graphene flakes dispersed into ZnO nanotubes and the dark current. Overall, simultaneous achievement of suppressed
CsPbCl3eCs4PbCl6 perovskite films (Huang et al., 2020; Zhu et al., dark currents and higher responsivity configures less NEP.
2020a). In the first concept of mechanism, photogenerated elec- To study the impact of structural and material integration on
trons or holes can be trapped at the surface adsorbents or by the photodetector performance, detectivity (D*) is also an essential
defect levels. While the other kind of photogenerated charge car- parameter. Moreover, it is anticipated to enhance the overall
riers (electrons or holes) circulates multiple times within the device photodetector performance. Specifically, two main factors such as
and generate photocurrent in the circuit. In another kind of noise developed and normalized SNR performance of the device
mechanism, charge carriers generate on the surface of adsorbents. can be revealed. Considering the above features, detectivity can be
Also, one kind of charge carriers diffuses into the material and estimated by using the following expression (Omnes et al., 2007),
contributes to current generation. The common concept in both
pffiffiffiffiffiffiffiffiffi
cases is surface adsorbents acts as a gate, which stimulates the ADf
photocurrent generation. The regime of photogating and photo- D* ¼ (3)
NEP
conducting effects is difficult to differentiate during the photode-
tector performance because of both phenomena happen in the At low short noise conditions detectivity can be written as,
same device. pffiffiffi
Rl A
D* ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffi (4)
1.1.3. Photovoltaic effect ð2eID Þ
A typical photovoltaic effect can be mainly observed during the
formation of PN, NPN, PNP, and at metal-semiconductor interfaces. where, Df, e, and ID are bandwidth, electronic charge, and dark
Therefore, the device architecture provides work function differ- current respectively.
ence, charge carrier gradient, and Schottky junctions. These fea- In addition to the above key features, external quantum effi-
tures lead to the formation of built-in electric field at the junction. ciency (EQE) is also a prominent factor. The EQE can be defined as
As a result, photogenerated electrons and holes can be effectively ratio between number of electron-hole pairs (contributed for
separated. This phenomenon allows successful nonlinear current- photocurrent generation) and total number of electron-hole pairs
voltage (IeV) characteristics. Specifically, the output is either produced (by absorbing the incident light). The following expres-
photocurrent or photovoltage. Considering the above effective sion is used to determine the EQE of photodetector (Omnes et al.,
photogenerated charge carrier separation under built-in electric 2007),
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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

2.1. ZnO-based photodetectors

hcRl
EQE ¼ (5)
el Among various metal oxide semiconductors, ZnO has been
extensively studied and used in various applications (Khan et al.,
where, h is the planks constant and l is the wavelength of the
2020; Saric et al., 2019; Shiau et al., 2020; Chauhan et al., 2020;
incident light. To study the impact of various nanostructures on the
Rabani et al., 2021). In particular, ZnO exhibit a wide bandgap
enhancement of photodetector performance (responsivity, detec-
(~3.2 eV) and n-type semiconductor behavior with exciton binding
tivity, noise equivalent power, and external quantum efficiency),
energy of ~60 meV (Pearton et al., 2003). Considering the wide
we explored the photodetector performance in UV, visible and IR
bandgap, ZnO importance significantly aided for the improved UV
region. Considering the above features, we extracted the superior
absorption. Note that engineering of ZnO UV photodetectors also
photodetector performance of various materials in UV, Vis and IR
involves superior charge carrier generation (electron-hole pair) and
regions.
separation. Driven by the above-mentioned constructive features,
we here attempted to explore various device fabrication techniques
2. Progress on UV photodetectors to reveal superior UV photodetector performance. In this section,
M-S-M structured Pd and Ti doped ZnO films have been demon-
Photodetection in UV region draws undivided extension due to strated for better understanding the possibility of Schottky and
its ability in diverse applications: (i) flame and radiation detection ohmic contacts formation for superior UV photodetector
to take preventive measures, (ii) astronomical studies and secured performance.
space communications, (iii) environmental and biological studies, The role of thermal evaporation and sol-gel deposition tech-
(iv) chemical analysis for screening, and (v) optical communica- niques has been highlighted to achieve superior UV photodetector
tions (vi) missile plume detection etc. In particular, typical UV ra- properties of ZnO thin films under Schottky junction formation (Ali
diation categorized into four main spectral regions such as UV-A and Chakrabarti, 2012) In this study, a key factor for superior UV
(400 nme320 nm), UV-B (320 nme280 nm), UV-C photodetector performance of ZnO thin films compared by
(280 nme200 nm), and far UV (200 nme10 nm) (Ren et al., considering the deposition techniques. The sol-gel derived ZnO
2013). It should be highlighted that UV light (˂ 280 nm) cannot thin film photodetectors exhibited superior responsivity (0.17 A/W)
penetrate into the earth’s atmosphere. Interestingly, previous and EQE (62%) compared to the thermal evaporated ZnO (respon-
studies show that most of the UV light reaching the atmosphere sivity of 0.08 A/W and EQE of 23%). It is to be highlighted that sol-
falls under UV-A category. Thus, detection of UV-A radiation gel technique is a feasible route to realize the adsorption and
detection become prominent (Reddy et al., 2019a,b; Yamada et al., desorption of H2O and oxygen. Thus, sol-gel derived ZnO thin films
2019; Yadav et al., 2019; Wang et al., 2019; Yadav et al., 2021). have prevailed superior photodetector properties compared to the
Over a period of time wide range of materials such as perovskites, thermal evaporated samples.
silicon derivatives, metal halides, transition metal dichalcogenides, Chemical bath deposition (CBD) method also guided to develop
and metal oxides have been developed to detect the UV light (Li stable ZnO films. After that, UV photoconductive behavior of ZnO
et al., 2020; Shi et al., 2016; Ahmadi et al., 2017; Mu et al., 2017; films (at 70  C) studied under the precise M-S-M structure forma-
Tian et al., 2015). Specifically, Si, SiC, diamond-based, nitride-based, tion (Shaikh et al., 2016). Specifically, the ZnO deposition time can
transitional metal oxides, and metal di-chalcogens used to detect be modulated to improve the UV photodetector performance. Here,
the UV radiation (Konstantatos et al., 2010, 2012). For better UV Ag metal used as electrode material. In this regard, the fabricated
photodetection and extensive period, photomultiplier tubes were Ag/ZnO/Ag (M-S-M structure) device architecture exhibited supe-
utilized under compact size. rior photocurrent generation (113.83 mA) and responsivity (28.14 A/
Nowadays, significant research is focusing on the fabrication of W) under UV light intensity (l ¼ 365 nm) of 1.8 mW/cm2 at applied
portable and highly sensitive UV detectors due to its rapid usage in bias of 5 V. Moreover, as the dependence of CBD technique on ZnO
microelectronic devices. Owing to the significant capability of UV thin film deposition, the photodetector stability and reversibility
absorption, several silicon-based materials have been extensively can be significantly improved with a rise time of 9 s and a fall time
used in various fields. However, silicon exhibits a bandgap of 1.1 eV, of 21 s. On the other hand, enhanced photoresponse attributed to
which make it to absorb visible radiation. To avoid that, several the improved crystalline nature of ZnO films (as deposited for 7 h)
layers of high-pass optical filters have been strategically intro- and interconnected wire structured morphology. At higher depo-
duced, which suggests the expensive device fabrication process. sition time, ZnO films peeled off easily. Considering the CBD tech-
Particularly, insertion of filters possesses relatively high noise nique and deposition time, it mean that superior charge carrier
generation (Chen et al., 2020a). Therefore, transition metal oxides, (electrons) transportation effectively observed at the metal-
SiC, and AlGaN alloys especially attractive for UV photodetection semiconductor interface.
under its chemically and thermally stable nature. Interestingly, Sol-gel technique is also beneficial for the fabrication of ZnO-
bandgap of above all materials falls under UV light, suggesting that based M-S-M Schottky barrier UV photodetectors (Ali et al.,
we can avoid the usage of high-pass optical filters (Chen et al., 2014). In this work, the photoresponse of pure ZnO, Pd doped
2020a). In another direction, metal oxide-based semiconductors ZnO, and Pd microplate embedded ZnO films have been compared,
such as ZnO, SnO2, Ga2O3, WO3, and TiO2 established as an excellent while Pd used as a Schottky-contact. Here, barrier-height and
UV photoactive material in optoelectronic devices. The above wide saturation current density of M-S-M photodiode were extracted
band gap metal oxide materials establish outstanding processing using logarithmic reverse current dependence. The Pd metal
approaches such as ease fabrication, scalability, control over crystal microplates incorporated with ultra-thin ZnO films showed higher
orientations, uniformity, and reproducibility in the UV photode- responsivity (0.33 A/W) and EQE (115%) under UV illumination
tector community. In such a way, all of the above features (360 nm). Whereas undoped ZnO (0.15 A/W and 52%) and PdeZnO
demonstrate that metal oxide semiconductors (ZnO, SnO2, Ga2O3, films (0.20 A/W and 70%) exhibited reduced responsivity and EQE
WO3, and TiO2) can be widely used in highly sensitive UV respectively than compared to the Pd microplate embedded ZnO
photodetectors.

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

films. The above results suggested that Pd microplate embedded

ZnO exhibit superior UV photodetector under depletion region
formation at the interface of microplates and semiconductor
interface.
In another direction, simple spray pyrolysis technique was
adopted to improve the UV photodetector performance of ZnO thin
films under Ag metal as an electrode (Inamdar et al., 2014). Under
forward and reverse bias conditions, IeV characteristics confirmed
the ohmic-contact formation of between Ag metal and ZnO. It
should be noted that UV photodetector performance of ZnO was
completely under visible-blind. As a result, ZnO exhibited highest
responsivity of ~788 A/W under 375 nm of UV illumination. Overall,
superior photocurrent and photoresponse properties of ZnO mainly
due to the highly crystalline nature of ZnO and intrinsic donor
defects (oxygen vacancies and Zn interstitials). Such behavior also
observed by the ZnO thin films developed by the CBD method
(Shaikh et al., 2016).
In addition to the pure ZnO (Inamdar et al., 2014), researchers
further focused on development of transition metal doped ZnO (Ti-
doped ZnO) thin films by spray pyrolysis technique to investigate
the UV detection properties (Shewale et al., 2015). Here, photode-
tector performance of pure and Ti-doped ZnO films systematically
studied under Sn as a metal electrode contact, which developed the
M-S-M structural configuration on both ZnO and Ti-doped ZnO
samples. Accordingly, linear IeV characteristics of this M-S-M
structure under forward and reverse bias confirmed the ohmic Fig. 2. Schematic depictions of (a) device structure of ZnO nanowire-based UV
contacts between the metal (Sn) layers and semiconductor (Ti- photodetector and (b) response and recovery current curve at an applied bias of 2 V of
doped ZnO). At selective bias voltage of 5 V, superior photocurrent a ZnO nanowire (Ates et al., 2012).
generation of 112.68 mA was observed for the Ti-doped ZnO under
UV illumination (l ¼ 365 nm), which is higher than dark state
2.2. SnO2-based photodetectors
(6.10 nA). At the same time, the responsivity was about 0.051 A/W
under the light intensity of 2 mW/cm2. In conclusion, it has been
Apart from the ZnO, SnO2 also found its importance in UV PDs
found that Ti metal doping significantly improved the charge car-
application and it behaves like a transparent metal oxide semi-
rier density in the ZnO, which yielded superior UV photodetector
conductor. It is generally agreed that SnO2 exhibits chemically and
performance.
thermally stable nature at atmospheric conditions (Wang et al.,
Low-cost solution processed method has been established to
2018). On the other hand, SnO2 is highly transparent to the
develop the ZnO nanowires for studying the UV photodetector
visible spectrum and reflects most of the IR radiation. Thus, SnO2 is
performance (Ates et al., 2012). Single-walled carbon nanotubes
suitable for transparent heat reflective surfaces (Pandey et al.,
(SWNT) layer was used as electrode onto the ZnO nanowires.
2020). Due to its transparent nature, SnO2 was vastly used in
Fig. 2(a) presents the schematic representation of SWNT thin films/
LCDs, LEDs, plasma display panels, and flat touch panels
ZnO nanowire photodetector. Here, various experimental studies
(Ramarajan et al., 2020). Apart from the above optoelectronic de-
conducted to reveal the relation between photodetector perfor-
vices, SnO2 also investigated in photocatalytic activity and active-
mance and nanowire density. These studies suggest that photo-
anode material in Li-ion batteries (Zhang and Wang, 2020). In
currents were significantly improved by increasing the nanowire
this section, we systematically discussed the development of SnO2-
density and maximum photocurrent shown was 520 mA under
based composites for enhancing the stability and overall UV
365 nm of UV light. As a result, SWNT thin films/ZnO nanowire
photodetector performance.
photodetector exhibited lower recovery time about 16 s (Fig. 2(b)),
Recently, SnO2 nanowire networks have successfully synthe-
which is ascribed to the improved charge carriers. Unlike the other
sized using CVD technique, which followed the vapor-liquid-solid
ZnO thin film photodetectors, transparent ZnO nanowires devel-
mechanism (de Araujo et al., 2020). Here, M-S-M based structure
oped on flexible substrates exhibited stable UV photodetector
was demonstrated neither by expensive photolithography nor in a
performance even under different radii of curvature.
clean room atmosphere. Specifically, the photodetector perfor-
Among the above discussed ZnO based PDs, spray deposited
mance of SnO2 nanowire network studied under various excitation
ZnO thin film PDs (M-S-M structure) achieved superior respon-
sources such as (i) UV lamp (2 mW/cm2) at wavelengths of 254 nm
sivity about 788 A/W upon 375 nm UV illumination, compared to
and 365 nm, (ii) white light (9.5 mW/cm2), and (iii) direct sun light
other ZnO based PDs. It was mainly due to the negligible dark
(78.6 mW/cm2). Upon UV illumination, SnO2 observed with supe-
currents under intrinsic donor defects, oxygen vacancies, and
rior photodetector performance with rise time (tr) of 0.37 s and fall
interstitial Zn. On the other hand, ZnO NWs were exhibited supe-
time (tf) of 0.59 s at 5 V bias voltage. It has been found that rise time
rior photocurrent about 520 mA under UV illumination of 365 nm
and fall time increased in the case of sun light (tr ¼ 0.61 s and
wavelengths and comparable responsivity of 0.15 A/W than other
tf ¼ 0.55 s) and white light (tr ¼ 71.6 s and tf ¼ 131.5 s) conditions.
ZnO PDs. It should be highlighted that high surface to volume ratio
Apart from this, high sensitivity (>104) was obtained under UV
of ZnO NWs resulting in higher photo absorption.

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

light compared to the outdoor measurements. It concluded that oxygen absorption and desorption for achieving the smooth
SnO2 prevailed superior UV photodetector performance. transfer of charge carriers under UV illumination. The band to band
Similarly, vertically aligned SnO2 NWs were successfully syn- charge carrier transition between the SnO2 hollow spheres is pre-
thesized by glancing angle deposition (GLAD) method (Chetri et al., sented in Fig. 3(b). The device performance was investigated both
2020). In this investigation, effect of annealing temperature (350  C, in vacuum and ambient atmosphere. Both dark and light currents
550  C, 650  C, 750  C, and 900  C) on structural, optical, and were higher in the vacuum conditions due to the reduced gas
electrical properties of SnO2 NWs systematically studied. In such a pressure. The linear IeV curves of the device revealed the ohmic-
way, the device fabricated at selective annealing temperature of contact formation. Moreover, the SnO2 hallow sphere film device
650  C achieved improved crystalline nature. Therefore, SnO2 NWs exhibits high sensitivity, stability and improved signal-to-noise
annealed at 650  C achieved superior photodetector performance ratio (SNR) about 300 times under the illumination of UV light of
with maximum responsivity of 2.58 A/W and photodetectivity of wavelength 320 nm at 45 mW/cm2 intensity. The enhanced sensi-
64.13  1010 Jones at l ¼ 300 nm of irradiance than other annealing tivity and SNR was attributed to the efficient photo-absorption by
temperatures. In a word, crystalline nature boosted the capacity of high surface to volume ratio SnO2 hallow spheres. The spectro-
defect controlling, which results to the increase of charge carriers. scopic photocurrent responds of the SnO2 device is depicted in
In addition to the above pure SnO2 NWs (de Araujo et al., 2020; Fig. 3(c) at different incident wavelengths. The photocurrent was
Chetri et al., 2020), SnO2-based heterojunction (ZnO/SnO2) core- found to be 1.5 nA at 320 nm of illumination. Overall, the obtained
shell nano-rod arrays (CSNAs) developed using facile hydrother- results attest that SnO2 is highly sensitive to the UV light.
mal and chemical liquid deposition techniques (Fu et al., 2020). From the above SnO2-based materials, ZnO/SnO2 core shell NRs
They highlighted the importance of localized excitons for recovery achieved superior photocurrents about 3.2 mA, which is 1000 times
of near-band-edge transition. Therefore, Iphoto/Idark ratio of ZnO/ higher than pure SnO2 NWs. It is to be highlighted that constructive
SnO2 ensured 7.2  104 at 1 V, which was ~270 times higher than interfacial interaction between ZnO and SnO2 resulted improved
pure ZnO. Further, with the introduction of localized states in the photon absorption and photocurrent generation. On the other
ZnO/SnO2, ZnO/SnO2 enhanced the photoresponse by means of hand, SnO2 nanospheres showed very low photocurrent about
responsivity (28.5 A/W) and specific detectivity (2.9  1014 Jones). It 1.5 nA. But, its dark to light photocurrent ratio was much higher,
is also improved in mitigating the response time of ZnO/SnO2 (8.7 s) which is also compatible with the flexible technology.
compared to ZnO (45.0 s). On the other hand, recovery time of ZnO/
SnO2 (20.8 s) also decreased compared to ZnO (56.6 s) under
nanocrystalline SnO2 shell-layer development on ZnO. 2.3. Ga2O3-based photodetectors
In another direction, superior photodetector performance was
achieved by developing the flexible hollow-sphere SnO2 photode- In addition to the ZnO and SnO2, Ga2O3 is also a promising
tector using water-oil interfacial assembling technique onto the transparent metal oxide semiconductor with a wide bandgap of
polyethylene terephthalate (PET) substrate (Tian et al., 2013). Under ~4.8 eV (Chen et al., 2018). In such a way, Ga2O3 diversely used in
specific hand-operable shadow mask, Cr/Au electrodes were the field of UV-optoelectronics, antireflective coatings, high-
deposited on the as-transformed SnO2 hollow-sphere nanofilm. temperature sensors, and solar cells (Guo et al., 2019; Xu et al.,
Fig. 3(a) represents the photodetector mechanism based on the 2020; Minami et al., 2013). Thus, we elaborately discussed the
importance and recent advancements in the Ga2O3-based UV

Fig. 3. Graphic representation of (a) oxygen-adsorption process under dark and oxygen-desorption process under UV-illumination of the SnO2 hollow spheres, (b) sphere-to-sphere
junction barrier for an electron transfer in the hollow sphere network, and (c) spectroscopic photocurrent responds of the device at different incident wavelengths (Tian et al., 2013).

6
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

photodetectors. 1000  C achieved remarkable responsivity of 20 mA/W, which was

Amorphous Ga2O3 (a-Ga2O3) was synthesized at different 500% higher than the Ga2O3 samples deposited at room RT (~7.5 mA/
deposition temperatures (RT-room temperature, 200  C, 300  C, W) as shown in Fig. 4(b). Moreover, lower dark currents about
400  C, and 500  C) for achieving the solar-blind deep UV photo- 0.0033 nA (at bias voltage of 5 V) achieved at 1000  C.
detector performance (Zhu et al., 2020b). In this study, higher ox- In summary, a-Ga2O3 based UV PDS showed superior respon-
ygen vacancies have been developed at higher deposition sivity of 138 A/W. It was mainly due to the high transparent nature
temperatures, which resulted in improved responsivity, wider of the amorphous Ga2O3. Whereas Mg-GaOx by showed respon-
detection range, and longer photo-decay time. Specifically, a-Ga2O3 sivity of 0.14 A/W, which was quite lower due to the increased
developed at selective deposition temperature of 500  C exhibited resistance. Here, Mg was used as a dopant in amorphous Ga2O3 to
superior photoresponsivity about 138 A/W compared to other reduce the interstitial defects and oxygen vacancies. On the other
temperatures of RT (1.46 A/W), 200  C (16 A/W), 300  C (25 A/W), hand, one-dimensional b-Ga2O3 nanobelts showed highest
and 400  C (71 A/W). Overall, deposition temperature played a key responsivity of 851 A/W than nanostructured single-Ga2O3 nano-
role to improve the UV photodetector performance of a-Ga2O3. sheets with a responsivity of 19.31 A/W. overall, these results
In addition to the a-Ga2O3 (Zhu et al., 2020b), highly-crystallized indicated that the better PD performance was produced by nano-
single b-Ga2O3 micro/nano-sheets were also studied to achieve structures of crystalline Ga2O3 films.
superior UV photodetector performance under Schottky barrier
formation (Zhong et al., 2015). Interestingly, b-Ga2O3 showed sig-
2.4. WO3-based photodetectors
nificant rectifying property under asymmetric contact formation at
an open circuit voltage of 0.33 V and UV wavelength of 254 nm. In
In spite of the above encouraging UV photodetector perfor-
such a way, b-Ga2O3 achieved remarkable photodetector perfor-
mance of various metal oxides, tungsten trioxide (WO3) is a tran-
mance such as sensitivity (dark current of ~10 nA), Rl (19.31 A/W),
sition metal oxide semiconductor with a bandgap of 3.2 eV (He
EQE (9427%), fast response time (about 20 ms), excellent stability et al., 2015). Primarily, the performance of WO3 extensively stud-
and reversibility. All these features pave a potential path towards
ied in the field of electrochromic devices owing to its thermal and
microwave device, high-speed integrated circuit, solar cells, and chemical stability. Thus, it has been used as dazzle-free mirrors in
photo-switches formation.
automobiles, variable reflection mirrors, and smart windows (Buch
In addition to the pure Ga2O3, Mg-doped amorphous gallium et al., 2016). It should be noted that WO3 also provides structural
oxide (Mg:GaOx) films exhibited remarkable solar-blind UV
transformation and non-stoichiometric phase transitions, which
photodetector (SBUV PD) performance (Zhang et al., 2019). Inter- ensured its importance precisely in optoelectronic sensors and
estingly, Mg:GaOx film highlighted with decrement in the trapping
display systems (Siciliano et al., 2008; Jain et al., 2021). Thus, we
centers for achieving the improved photo-generated charge car- explored the importance of UV photodetector performance of WO3
riers. Specifically, Mg:GaOx-based SBUV PD exhibited suppressed
and WO3-based materials.
dark currents (48 pA), higher light-to-dark current ratio Few-layered WO3 nanosheets were successfully fabricated to-
(~338 at 3 V bias voltage), and faster response (a decay time of
wards superior UV photodetector performance (Liu et al., 2015).
0.15 s) time. Thus, Mg-divalent ion dopant plays a key role in GaOx Here, WO3 nanosheets were synthesized by the CVD technique on
to achieve the lower dark-current and quick response time.
the Si/SiO2 substrate. Later, photolithography was used to develop
Thin films of poly-Ga2O3 was developed using sputtering tech- the patterns and Cr/Au metal electrodes were deposited using e-
nique on c-plane sapphire substrate followed by the thermal
beam deposition. Therefore, WO3 nanosheets exhibited superior
annealing at 800  C, 900  C, 1000  C, and 1100  C (Hu et al., 2020). photoresponse (293 A/W) and EQE (997%) under UV light
Later, Ti and Ni metal electrodes were developed on poly-Ga2O3
(l ¼ 365 nm). It is further established that the photocurrent gen-
thin films. Consequently, M-S-M device structure was achieved as eration under switching on and off cycles was quick and stable.
shown in Fig. 4(a). In particular, Ga2O3 thin films annealed at
Here, the Iphoto/Idark ratio was observed with 2000, which expected
1100  C temperature showed less responsivity and photocurrent
to develop ultrafast WO3 based optoelectronic devices.
than the as deposited samples. This was due to recrystallization and
As WO3 nanosheets revealed very high responsivity under UV
diffusion of Al from the substrate into Ga2O3 films caused wide
illumination, another group developed WO3 monolayer by atomic
bandgap energy of 5.10 eV, which is higher than the incident UV
layer deposition (ALD) onto the Si wafer to evaluate its UV PDs
energy to generate photocurrent. However, Ga2O3 films annealed at
performance as shown in the (Hai et al., 2017a). Unlike the thin film

Fig. 4. Device structure representation of (a) M-S-M structured Ga2O3-based UV photodetector (Hu et al., 2020) and (b) responsivity behavior as a function of incident wavelength
(UV-light) for the poly-(AlxGa1-x)2O3 photodetectors at bias voltage of 5 V.

7
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Fig. 5. (a) WO3 photodetector fabricated through ink print on SiO2/Si wafers with Au electrodes and (b) dark and photocurrent response at different bias voltages of WO3-based
photodetector under UV-illumination (Cook et al., 2018).

based WO3 PDs (Yadav et al., 2019), monolayer of WO3 exhibited 2.35  1010 W and detectivity 1.34  109 Jones).
ultra-fast response (~2.5e2.7 ms) while maintaining long-term Building upon the above WO3 based PDs, the pleasant surprise is
stability for about 250 cycles. The simple design of monolayer that nanosheets showed excellent responsivity of 293 A/W, which
semiconductor oxide enhanced the dynamics of photon- was higher than that of other WO3 based UV PDs discussed. In
semiconductor interactions without many losses due to the elec- another creative study, few layers of WO3 nanosheets out-
tron backscattering which is usually observed in multilayered performed the photodetector performance compared to the mon-
nanostructures. In addition to this, ohmic-contact between the olayered WO3. Experimental realization revealed that band gap of
photoactive material and electrode as shown in also assisted in few layered WO3 nanosheets confined to the UV region (365 nm),
enhancing the photocurrent. Fig. 5(a) shows the inkjet printed WO3 which stimulated the overall photodetector performance.
thin film developed onto the SiO2 substrate based UV photode-
tectors and Fig. 5(b) exhibits the evidence of ohmic-contact be-
tween the electrode and photo-active material (Cook et al., 2018). 2.5. TiO2-based photodetectors
Even though, both ink jet printed WO3 thin films and ALD syn-
thesized mono-layer of WO3 consists of ohmic-contact, the mono- To prove the viability of TiO2 on various applications, re-
layer of WO3 was exhibited the higher responsivity of 71.6 A/W searchers focused on the photocatalysis, Li-ion batteries, solar cells,
than inkjet-printed WO3 thin film (2.70 A/W). It was due to the photodetectors, and self-cleaning surface coatings (Cho et al., 2021;
efficient charge transfer by 2-D structured WO3 device. Yan et al., 2017; Kment et al., 2017; Zheng et al., 2016; Patrocinio
Implying a similar device concept, monolayer structured WO3 et al., 2014). It is particularly important to prove and understand
demonstrated for revealing the photodetector performance in UV- the UV photodetector performance. We briefly note that TiO2 is a
A region with strategic functional capabilities (Hai et al., 2017b). It is transitional metal oxide, comes with a bandgap of (3.2 eV) and
important to note that the precise role of monolayer structured exhibits rutile, anatase, and brookite crystalline forms ( Zhao et al.,
WO3 achieved ultrafast photoresponse time (<40 ms) and photo- 2007). However, one must consider the chemical inertness, high
responsivity (~0.329 A/W). The above achieved response time was photocatalytic activity, strong oxidizing power, endurance, non-
superior to the earlier reports on WO3-based UV photodetectors. toxicity, and low fabrication cost of TiO2 (Hitosugi et al., 2010;
Also, monolayer WO3 responded quickly under UV-A light Bera et al., 2018). Thus, TiO2 also inspired by the excellent structural
compared to most of the other 2-D ultrathin nanomaterial photo- transformation and non-stoichiometric phase transitions, which
detectors. Specifically, monolayer structure certainly possesses safeguarded its importance in optoelectronic sensors and display
quantum-confined effects and new functional opportunities to systems. In the following discussion, we systematically discussed
power the various optoelectronic devices. Because the monolayer and examined the importance of TiO2-based UV photodetectors.
WO3 processes new path for the fabrication of highly flexible, Nanocrystalline M-S-M structured Au/TiO2/Au thin films were
inexpensive, and extremely sensitive photodetectors, it is reason- fabricated by the sol-gel technique (Xue et al., 2007). The above
able to expect these types of UV photodetectors in industrialization device structures highlighted the importance of dark currents in
and commercialization. the order of nA (1.9 nA) and photoresponsivity of 199 A/W under a
The popular M-S-M device structure is successfully synthesized wavelength of 260 nm (at 5 V bias voltage). Taken together, high
by stacking the WO3 nanospheres and WO3 thin films on sapphire responsivity being made by the existence of neutral photo-
substrates (Lee et al., 2018). The dominant noise source of the M-S- conductor region and reduced Schottky barrier. The Au/TiO2/Au M-
M UV photodetector was flicker noise. The UV photodetector per- S-M structure showed defects trapped in the nanocrystal has been
formance of M-S-M structured WO3 nanospheres/WO3 thin film widely distributed. These widely distributed defects acted as the
was higher than thin film structured WO3 M-S-M photodetector. recombination centers, which were eventually resulted in the
The above features determine the strength of high surface-to- decrement of response time (rise time of 6 s and decay time of 15 s).
volume ratio of WO3 nanospheres. Accordingly, WO3 nanosphere/ Overall, all the above features (reduced recombination, defect
WO3 thin film M-S-M device architecture (at a wavelength of trapping and lower response time) attributed to the improved
350 nm) achieved superior photoresponsivity (89.2 mA/W), noise crystalline nature of the TiO2 nanocrystals.
equivalent power (6.10  1011 W), and detectivity (5.19  109 Similar M-S-M device structure also studied on RF magnetron
Jones) compared to the M-S-M structured WO3 thin film photo- sputtered TiO2 thin films (Caliskan et al., 2013). Here, Pt/Au metal
detector (photoresponsivity-20.7 mA/W, noise equivalent power- electrode contacts used to develop the M-S-M device structure.
With the development of M-S-M device structure, avalanche effect
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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

and high electric field between the electrodes significantly influ- achieved. Accordingly, the device responsivity significantly
enced the exponential growth of dark current. As a result, M-S-M improved by 80% with extremely low dark-currents (~50 pA)
based photodetector helpful for the achieving the very low dark compared to the traditional TiO2 UV-PDs (~20 mA). Bringing
currents about 1.57 nA/cm2 at 5 V. The results show that the TiO2 together, the optimized TiO2/Ag/TiO2 device exhibited outstanding
M-S-M photodetector at specific bias voltage of 50 V and wave- UV responsivity of 0.2 A/W, detectivity of 5.3  1013 Jones and Ion/
length of 300 nm achieved the responsivity of 1.73 A/W. Also, the Ioff ratio of 137.2 dB, even under self-powered operating mode upon
response time of the photodetector was measured under the rise 365 nm monochromatic UV light illumination.
and fall time of 7 s and 3 s, respectively. It can be attributed to the Considering the TiO2 based UV photodetectors, TiO2 nano-
increased trap density existing in the as-deposited films and crystalline films (Au/TiO2/Au) achieved remarkable responsivity
limited space between metal contacts and photo-active material. (199 A/W) under the wavelength 260 nm of UV light. It was pri-
To further study the importance of M-S-M structure, epitaxial marily due to the improved crystallinity and reduced Schottky
TiO2 thin films were deposited on LaAlO3 single crystal substrates barrier height. However, TiO2 thin film and TiO2 epilayer based PDs
by RF sputtering technique (Xing et al., 2011). Here, Ag metal exhibited comparatively low responsivity of 3.63 A/W (310 nm) and
contacts were developed on the epitaxial TiO2 layers and Ag/TiO2/ 0.21 A/W (270 nm), respectively. Besides, the TiO2 based materials
Ag UV PD test device has been fabricated. Accordingly, the M-S-M raised its importance as a UV-A sensitive nature and preferred for
based TiO2 photodetector exhibited the superior responsivity of environmental applications.
3.63 A/W at a UV wavelength of 310 nm. In order to achieve the In the above sections, we have explored the strategic ap-
ohmic-contact behavior in M-S-M photodetector, it is necessary to proaches to fabricate the UV photodetectors using various metal
use the high work function Ag metal as electrode. Because of oxide semiconductors (ZnO, Ga2O3, SnO2, TiO2, and WO3). Specif-
ohmic-contact behavior, M-S-M structure proved reduced dark ically, experimental conditions such as deposition time, metal
currents about 0.14 nA at a bias voltage of 10 V. contacts and annealing temperature greatly devoted to achieving
Implying a similar concept, high-quality TiO2 epilayers were superior UV photodetector performance. By comparing the
developed on the lattice-matched LaAlO3 substrates at 500  C using annealing temperature, Ga2O3 films annealed at 600  C achieved
pulsed laser deposition technique (Zhang et al., 2015). A prototype excellent responsivity of 138 A/W compared to the SnO2 annealed
of M-S-M based Au/TiO2/Au UV-photodetector device was fabri- at 500  C (2.58 A/W). Indeed, doping effect predominantly influ-
cated using Au as Schottky-contact. Here, the as-deposited TiO2 enced the dark current of Pd doped ZnO and Mg doped Ga2O3 films.
thin film exhibited excellent visible-blind UV characteristics with Especially, the flexibility of UV nanostructure photodetectors
an optical bandgap of 3.25 eV, signifying its potential in UV (nanowires and nanospheres) appeared to reduce the dark cur-
detection. As a result, this M-S-M based TiO2 UV-photodetector rents. But, the responsivity was low due to the increased recom-
device architecture had been proven as a high UV to visible rejec- bination rate. However, the responsivity of the UV photodetector
tion ratio of 105 under low dark-currents (0.25 pA at 5 V) and high drastically increased to 28.5 A/W by introducing the bi-layer of
responsivity (0.21 A/W) upon UV illumination of wavelength ZnO/SnO2. It was due to the formation of optimized heterojunction
270 nm. Such a low dark current value reveals the Schottky junc- interface and smooth flow of photogenerated charge carriers.
tion formation at the interface of metal/semiconductor. Among all the metal oxides, WO3 films deposited (CVD technique)
Unlike the pure TiO2, another TiO2/Ag/TiO2 tri-layered structure achieved high responsivity (293 A/W) and Iphoto/Idark ratio (2000).
fabricated using GLAD technique to realize the self-powered Overall, taking the benefits of optimized experimental conditions,
photodetector under dissimilar top electrodes (Ferhati et al., appropriate doping element and developing of bi-layers signifi-
2020). The optical activity of multilayered TiO2/Ag/TiO2 was first cantly influenced the photodetector performance of WO3. Consid-
optimized using the genetic algorithm global optimization tech- ering the above key features, we summarized the UV photodetector
nique, where outstanding UVeVis absorbance behavior was performance of various metal oxide semiconductors (ZnO, Ga2O3,

Table 1
Photodetector performance comparison under UV illumination with different semiconducting metal oxides.

Material Methodology Photocurrent (mA) Responsivity (A/W) Detectivity (Jones) EQE (%) Ref

ZnO Sol-gel 1.35 0.17 e 62 (Ali and Chakrabarti, 2012)

ZnO Chemical bath 113.8 0.33 e 115 Shaikh et al. (2016)
PdeZnO Sol-gel e 0.14 e e Ali et al. (2014)
ZnO Spray pyrolysis e 788 e e Inamdar et al. (2014)
TieZnO Spray pyrolysis 112.68 0.051 e Shewale et al. (2015)
ZnO NW Spin coating 520 e e e Ates et al. (2012)
SnO2 NW CVD 25 e e e de Araujo et al. (2020)
SnO2 NW GLAD e 47.9 64.1  1010 1.0  102 Chetri et al. (2020)
ZnO/SnO2 Hydrothermal 3.22  103 28.5 2.9  1014 e Fu et al. (2020)
SnO2 spheres Interfacial assembling 1.5  103 e e e Tian et al. (2013)
Ga2O3 RF sputtering 111 138 e e Zhao et al. (2020)
Ga2O3 CVD 2.8 19.31 e 9.4  103 Zhong et al. (2015)
Mg:GaOx e e e e e Zhang et al. (2019)
Ga2O3 RF sputtering 12  1011 20  106 e e Hu et al. (2020)
WO3 NS CVD ~25 293 e 9.9  102 Jain et al. (2021)
WO3 monolayer ALD 15.1  103 71.6 e 1.13  104 Hai et al. (2017b)
WO3 monolayer ALD 900 0.329 e e Hai et al. (2017c)
WO3 NS VCCS e 0.089 5.19  109 e Lee et al. (2018)
TiO2 Sol-gel 2.3 199 e e Xue et al. (2007)
TiO2 RF sputtering ~1 1.73 e e Caliskan et al. (2013)
TiO2 RF sputtering 48 3.63 e e Xing et al. (2011)
TiO2 PLD 1.0 0.21 e e Zhang et al. (2015)
TiO2/Ag/TiO2 GLAD 100 0.2 5.3  1013 e Ferhati et al. (2020)

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

SnO2, TiO2, and WO3) in Table 1. rGO) as a bi-layer revealed the visible photodetector performance
(Chowdhury et al., 2020). Specifically, PQD/rGO structure describes
3. Research progress on visible photodetectors the advantage of negatively charged functional groups present on
the rGO surface for the diffusion of electron cloud, nucleation, and
Despite the significant advantage and importance of UV pho- growth of PQDs on rGO. As a bilayer formation of PQD/rGO, desired
todetectors based on wide band gap materials in field of environ- charge transfer occurs from PQDs to rGO compared to the PQDs and
mental monitoring, flame detection and controlling, visible PDs rGO mixture as a thin film using spin coating or drop-casting
also have numerous applications in the contemporary world of method. The precise development of PQD-rGO exhibited high
technology in the following aspects: (i) collision detectors for responsivity (1.07  103 A/W), detectivity (1  1013 Jones), and
monitoring hurdles in driver bling spot, detectors for controlling air sharp switching in the visible region. Fig. 6(a) and (b) depict the
bags opening timings in usage in automotive technology and (ii) schematic representation of GPQD-rGO photodetector and energy
also in ultra-fast imaging technology. With the emergence of visible band alignment, which reveals the charge transfer from GPQD and
light photodetectors, it is essential to understand the visible light rGO. Fig. 6(c) illustrates the transient photoresponse of GPQD-RGO
photodetector mechanism and performance to reach the current superstructure under light illumination (442 nm) with On and Off
technological requirements. Primarily, previous reports on silicon conditions for one cycle. From the spectrum, fast photoresponse
and germanium based materials highly suitable for visible light was observed with quick rise time (0.3 s) and fall time (0.3 s). As the
photodetector performance due to its narrow bandgap PQDs normally grown on rGO, low responsivity was achieved due
(Konstantatos et al., 2007; Yang et al., 2017, 2018; Wang et al., 2014, to the poor charge transfer at the interface. Therefore, the direct
2015; Flemban et al., 2017; Xue et al., 2011; Siontas et al., 2019). It growth of PQDs on the rGO sheets could be adopted for develop-
should be noted that visible light photodetectors exhibit higher ment of stable visible light active 2-D photodetectors like transition
response time, poor sensitivity, high dark current and relatively low metal halides and metal dichalcogenides.
EQE compared to UV photodetectors. Recently, investigation on gallium nitride (GaN) and nitrogen-
Interestingly, great efforts have been devoted on lead dihalide doped single-layer graphene (N-SLG) heterostructures endeav-
(LDH) and transition metal dichalcogenides to achieve the superior ored to reveal the visible photodetector performance
visible light response (Velusamy et al., 2015; Wu et al., 2016a; (Sankaranarayanan et al., 2020). In this work, the GaN epilayer was
Zhang et al., 2016; Lin et al., 2015; Ramasamy et al., 2016). It should deposited on N-SLG substrates using CVD technique. They selected
be noted that these materials are very susceptible to react with the Au as a metal contact, which associated for developing the M-S-M
environmental oxygen. However, PbI2 and PbFI show excellent structured photodetector. Experimental results, further suggest
response under vacuum conditions (Ismail et al., 2019; Wei et al., that the M-S-M structure formation prevailed superior responsivity
2017; Wang et al., 2017). Very recently (Shkir et al., 2019), re- and detectivity in the range of 150e400 A/W and
ported cadmium zinc telluride (CZT) and indium-doped CZT 1.08  1012e2.89  1012 Jones, respectively. Confirming the supe-
(InCZT) single crystals-based visible light photodetectors with high rior visible light response, the M-S-M structure further observed
responsivity. On the other hand, two-dimensional (2D) graphene with the rising time and fall time of 10 ms and 25 ms, respectively.
(rich of carbon atoms) came into limelight. Thus, it has been used in Overall, the GaN epilayer deposited on N-SLG substrate were highly
numerous fields including solar cells, sensors, and optoelectronics. prompt to the visible light with an improved charge carrier
Indeed, graphene with packed carbon atoms exhibit superior me- mobility and charge carrier generation.
chanical strength, high electron conductivity, broad range spectral Usually graphene oxide (GO) provides superior charge carrier
absorption, and ultra-high mobility (Falkovsky, 2008; Balandin, mobility for further development in the visible light photodetector
2011; Papageorgiou et al., 2017; Neto et al., 2009). In the photo- performance. In such a way, graphene oxide doped lead iodide (GO-
detector filed, inherent structural stability describes the improved PbI2) studied for achieving the visible light photodetection perfor-
overall photodetector performance. Considering the above mance under 532 nm (Sharma et al., 2020). In this study, PbI2
constructive features, we explored the importance of 2D graphene- nanorods/GO heterostructure was synthesized via microwave-
based and other heterostructures towards visible light photode- assisted synthesis route. As the influence of GO doping, the
tector performance. photodetector performances of GO-PbI2 such as Rl, EQE, and D*
were significantly increased (0.182 A/W, 42%, and 1.79  1011 Jones)
3.1. Graphene based visible photodetector compared to the pure PbI2 (0.060 A/W, 14%, and 6.38  1010 Jones).
It is to be highlighted that the GO-PbI2 mainly provides the trap
Recently, cadmium zinc selenide nanostructures and rGO were centers at the interface, which filled under visible light illumina-
prepared separately and then mixed together as a solution in a tion. It can be attributed to the superior charge carrier mobility of
Teflon beaker containing glass substrate. Then the CZS-rGO nano- GO in the GO-PbI2.
composite thin films were deposited on the substrate through On the other hand, metallic (1T) configuration WSe2 from
hydrothermal-assisted chemical bath deposition technique for transition metal dichalcogenides family also exhibited highly effi-
revealing the visible light photodetector performance (Mathew cient visible photodetector performance with the integration of
et al., 2020). Here, the authors investigated the photodetector rGO (He et al., 2020). The nanostructures were systematically
performance under effective active area of 0.5 cm2, where silver synthesized using modified-hydrothermal process. The results
paste was used as an electrode material. In this study, the device showed that rGO/WSe2 achieved remarkable photodetector per-
performance was significantly increased under selective rGO con- formance under improved (i) photocurrent generation by the 1T-
centration of 2 wt%. The results showed that rGO-CZS achieved configuration WSe2 and (ii) charge carrier mobility of rGO, which
superior visible light responsivity (18.5 mA/W) and specific proving efficient charge transfer at the interface of rGO/WSe2.
detectivity (2.08  1012 Jones). Most importantly, the rGO sheets Accordingly, rGO/WSe2 exhibited superior photoresponsivity (~105
included in this device contributed to superior charge carrier A/W) compared to the pure WSe2 (~89 A/W) under visible light of
mobility, which eventually reduced the transit time. In a word, rGO- wave length 540 nm. In such a way, the time taken for light
CZS represent the strength of visible light responsivity under the response of rising and decay were 0.001 s and 0.002 s respectively.
community of rGO sheets. Thus, the rapid raising and decay of photocurrents of rGO/WSe2
Novel perovskite quantum dots (PQDs) developed on rGO (PQD/ describes the capability of improved electrical conductivity under
10
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Fig. 6. (a) Graphic of the GPQD-RGO photodetector, (b) energy band diagram of GPQD-RGO sample, and (c) transient photoresponse of ON and OFF conditions for one cycle under
light illumination of 442 nm (Chowdhury et al., 2020).

Fig. 7. (a) Schematic graphene/p-type doped-GeSn device, (b) enhancement factor of photocurrent for graphene/n-GeSn and graphene/p-GeSn as a function of excitation wave-
length; energy band diagram during (c) without laser and (d) with laser illumination on graphene/p-type doped-GeSn device (Lv et al., 2020).

11
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

the constructive interface-induce effect between WSe2 and rGO in MoS2 using two-step CVD method (Yuan et al., 2019). In this study,
the rGO/WSe2. In addition, rGO/WSe2 photodetectors provided an the CdSe/MoS2 photodetector was developed on the SiO2/Si sub-
intense spectral response in the UVevisible region (300e700 nm) strate. Moreover, the photodetector activity studied under the
than in longer wavelengths. development and patterning of Ti/Au metals using electron beam
Very recently, graphene/doped GeSn vertical heterostructures evaporation and electron beam lithography, respectively. Under
reported for its favorable visible photodetector performance (Lv constructive interface between CdSe and MoS2 in the CdSe/MoS2
et al., 2020). Specifically, they developed the monolayer graphene heterostructure, ultra-fast photoresponse time of ~370 ms and high
on doped GeSn. Fig. 7(a) presents the basic structural design of photoresponsivity of 12 A/W were achieved under visible light
graphene/doped GeSn photodetector. It was found that photo- illumination (upon 637 nm). Thus, CdSe/MoS2 composite was
generated charge carriers significantly separated and transferred prevailed another interesting feature such as efficient charge car-
after addition of graphene monolayer. The enhancement in the rier transportation. On the basis of above features, CdSe/MoS2 can
photocurrents under various wavelength regions is shown in act as an emerging visible light photodetector.
Fig. 7(b). It should be noted that the enhancement was relatively Combining of different sulfide materials is also a challenging
increased with the laser wavelength in n-type GeSn photodetector task for studying the visible light photodetector performance. Thus,
compared to the p-type GeSn. Accordingly, Fig. 7(c) depicts the SnS/CdS heterojunction photodetector was successfully fabricated,
band alignment between graphene and p-type GeSn in the which works under the strategic pyroelectric and photoelectric
graphene/p-type GeSn heterostructure. Especially, under laser effects (Chang et al., 2020). During the fabrication of SnS/CdS het-
illumination, charge transportation occurred from p-type GeSn to erostructure, CdS nanorod arrays synthesized using hydrothermal
graphene (Fig. 7(d)). Under such constructive heterojunction for- process on the FTO substrate. Later, SnS nanoflakes were coated on
mation, the visible light responsivity was found to be 200 mA/W. It CdS. Finally, Au electrodes were deposited on SnS/CdS using ther-
is to be noted that the presence of graphene monolayer of gra- mal evaporation technique. Fig. 8(a) presents the schematic rep-
phene/doped GeSn composite can be not only acted as an electron resentation of heterostructured SnS/CdS photodetector developed
transport layer but also provided a broadband photodetection from on FTO substrate. From the photoresponse perspective, SnS/CdS
532 to 1832 nm. nanostructure potentially studied as a function of time under
different visible light wavelengths (365 nm, 405 nm, 532 nm, and
3.2. Nanostructured based visible photodetectors 650 nm). From the Fig. 8(b), sharp spikes were observed under both
switching light on and off states, which was mainly due to the
Another transition metal dichalcogenides of MoS2 also pyroelectric effect. It is interesting to note that different
contributed its importance towards visible light photodetector pyroelectric-photoelectric effects observed in four stages. Fig. 8(c)
performance. In such a way, MoS2 combined with CdSe (CdSe/ illustrates the different mechanisms during the photodetector
MoS2). Here, CdSe nanoplates vertically assembled on monolayer performance. Under visible light, temperature gradient was

Fig. 8. Schematic (a) structural diagram of SnS/CdS heterojunction photodetector, (b) photoresponse as a function of time under different visible light illuminations, and (c)
fundamental working mechanism on the coupled pyroelectric-photoelectric effects (Chang et al., 2020).

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Fig. 9. (a) 3-D graphic drawing of Ag/MoSe2 NCs/ITO photodetector, (b) responsivity and EQE plots of Ag/MoSe2 NCs/ITO photodetector at different incident wavelengths, and (c)
carrier transport mechanism of the photodetector under Vb > 0 illumination condition (Patel et al., 2020).

established across the device as presented in stage-I. This temper- voltage > 0 V.
ature gradient leads to the pyroelectric current at first and then In addition to the above nanorod, nanoflakes and nanocrystal
disappeared when temperature gradient becomes zero. Thereafter, based visible light photodetectors, ultra-long catalyst-free WO3
photoelectric current prevails under light illumination in stage-II. nanowires (WO3 NWs) were synthesized using CVD technique to-
In the light off stage, the current goes to negative value and wards high-performance visible photodetector (Wang et al.,
comes back to zero in stage-III and IV. It should be highlighted that 2020b). In this system, WO3 NW was deposited on the SiO2/Si
extra pyroelectric current was mainly due to the internal pyro- substrate. The electrode pattern was designed by standard photo-
electricity of CdS nanorods. Accordingly, SnS/CdS nanostructure lithography method. Finally, Cu/Au electrodes were deposited using
device exhibited superior visible photodetector performance at low thermal evaporation technique. Accordingly, superior visible light
temperatures. Specifically, under visible light (650 nm and photodetector performance (responsivity of 19 A/W and detectivity
0.08 mW/cm2), the SnS/CdS nanostructure achieved the respon- of 1.06  1011 Jones) was achieved under 404 nm laser light of in-
sivity (10.4 mA/W), detectivity (3.56  1011 Jones), and response tensity 71.23 mW/cm2 at a bias voltage of 0.1 V. The superior
time (less than 30 ms) at 130 K. Overall, the SnS/CdS nanostructure photodetector performance is attributed to the formation of defect
strengthened visible light absorption under pyroelectric and pho- less nanowires, high crystallinity, and high surface-to-volume ratio
toelectric efficiency of nanostructured SnS nanoflakes and CdS (Zhu et al., 2016; Wen et al., 2016; Li et al., 2015; Cheng et al., 2017).
nanorods. In conclusion, favorable formation of graphene-based materials
Understanding of photodetector performance by developing the (doped and heterostructure based) and various nanostructured
low-dimensional nanostructures is also necessary compared to the materials are crucial for achieving the superior visible light
conventional thin films, which manifest the superior photodetector photodetector performance. Among these, graphene-based heter-
performance. In such a way, single-crystalline MoSe2 nanocrystals ostructure (GaN/SLG) achieved superior responsivity (400 A/W)
(NCs) were synthesized via liquid exfoliation method for achieving and detectivity (208  1012 Jones) compared to the CdSe/MoS2
the visible light photodetector performance (Patel et al., 2020). nanocomposite (responsivity of 10.04 mA/W and detectivity of
Here, the MoSe2 layer developed on the ITO substrate using elec- 3.56  1011 Jones). A prominent feature for attaining a high per-
trophoresis deposition (EPD) technique and Ag was used as elec- formance is ultra-high mobility of graphene. On the other hand,
trode material as shown in Fig. 9(a). Such a device fabrication led to nanostructure orientation of MoSe2 single crystal and WO3 nano-
the superior responsivity (566 mA/W) and EQE (155%) (Fig. 9(b)). wires also considered for achieving superior photodetector per-
Also, specific detectivity of 3.69  1011 Jones was achieved. These formance under visible light. Among all the above photodetectors,
results suggest the formation of ohmic-contact at the interface of WO3 NWs demonstrated commendable responsivity (19 A/W) and
Ag and MoSe2, which leads to the high electron density at the detectivity (1.06  1011 Jones). In a word, noteworthy feature of
surface states. Moreover, absorption and desorption of oxygen WO3 in nanowire structure provides potential feature as a
molecules facilitated many trap levels, which occupied by the graphene-free visible photodetector. Finally, photodetector per-
photogenerated charge carriers and avoided recombination rate. formance of various visible light photodetectors based on nano-
Fig. 9(c) illustrates the charge carrier transport mechanism of structure formation and graphene source compared in Table 2.
MoSe2 NCs photodetector under visible light (450 nm) at bias

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Table 2
Recent results on visible photodetector performance with different materials.

Material Methodology Photocurrent (mA) Responsivity (A/W) Detectivity (Jones) EQE (%) Ref

rGOeCZS Hydrothermal e 18.5  103 2.08  1012 e Mathew et al. (2020)

PQD-RGO Drop casting e 1.07  103 1  1013 e Chowdhury et al. (2020)
GaN/N-SLG CVD 16.5  103 400 2.89  1012 e Sankaranarayanan et al. (2020)
GO-PbI2 Microwave e 0.182 1.79  1011 42 Sharma et al. (2020)
RGO/1T-WSe2 Step Hydrothermal 90 105 e e He et al. (2020)
Graphene/GeSn MBE e 0.2 e e Lv et al. (2020)
CdSe/MoS2 CVD 10  103 12 e e Yuan et al. (2019)
SnS/CdS Hydrothermal 7.12 10.4  103 3.56  1011 Chang et al. (2020)
MoSe2 NCs Liquid exfoliation e 566  103 3.69  1011 155 Patel et al. (2020)
WO3 CVD e 19 1.06  1011 e Wang et al., (2020b)

4. Research progress on IR based photodetectors various QDIPs based on its charge transportation mechanism for
achieving superior IR light detection.
Unlike the UV and visible light photodetector, infrared (IR)
photodetectors are mainly employed in astronomy and defence
areas. In this situation, higher wavelengths are required to detect 4.1. InAs-based quantum dot infrared photodetectors
the objects and targets. Defence applications include distinguishing
decoys from actual missiles, locating landmines during aircraft In a bid to develop the IR photodetector, self-assembled 50
landing, and identification of warm targets against a warm back- layers of InAs QDs with 30 nm thickness of GaAs spacers separating
ground. The current video camera industry has been dominated by them was developed on the <100> GaAs substrate (InAs/GaAs
the basic charge coupled device (CCD) detector technology. How- QDIPs). Then, InAs/GaAs QDIPs were sandwiched between the
ever, the latest technological advancements in mass production of collector and emitter (Liu et al., 2001). By this method, InAs/GaAs
IR detectors led to include it in video camera applications as well. QDIPs attained responsivity about 0.1 A/W at an IR wavelength of
Therefore, it is necessary to develop the low-cost IR PDs with high- 5000 nm (80 K). Ideally, superior response range was provided by
end device parameters such as sensitivity, spectral selectivity, the QDIPs under reduced density of states. In doing so, QDIPs
working temperature, and peak wavelength (Zeng et al., 2013; responsible for the variety of possible transitions, it become crucial
Chakrabarti et al., 2004; Tezcan et al., 2003). Currently, HgCdTe- for the occupancy of QD states.
based IR photodetectors have been using in astronomical applica- Based on emerging IR photodetector of QDIPs, another com-
tions, which possess superior responsivity and ultra-low noise posite based on GaAs QDIPs (InAs/InGaAs/GaAs QDIPs) was devel-
detection in the long-wave infrared regime (LWIR) (Elliott, 1998). oped by molecular beam epitaxy (Kim et al., 2004). In this work,
But, high cost, non-uniformity over a large area, and lack of avail- different monolayer (ML) QDs such as InAs(2-ML),
ability of substrates are the limitations associated with the HgCgTe- In0.15Ga0.85As(20-ML) and GaAs(130-ML) have been utilized to
based IR detectors (Rogalski, 2005). To overcome, InAs-(IneGa)Sb develop the InAs(2-ML)/In0.15Ga0.85As(20-ML)/GaAs(130-ML) het-
based IR photodetectors were developed as alternative to the erostructure. The resultant composite sandwiched between highly
HgCdTe-based detectors, which showed promising features due to Si-doped GaAs as top and bottom contacts. Notably, the InAs/
their low dark-currents and high quantum efficiency (Claro et al., InGaAs/GaAs QDIPs framework exhibited superior detectivity about
2020; Wu et al., 2016b; Pan et al., 1998). Moreover, employing Si 33  1011 Jones at 9.3 mm IR wavelength. Also, extreme low noise
and InSb based materials are predicted to outperform the very (1014 A/Hz1/2) was observed at 1.4 V and 78 K, which were higher
long-wave infrared regime (VLWIR) and mid-wave infrared regime than the previously reported QDIPs (mention the value) (Ye et al.,
(MWIR) performance (Tran et al., 2019; Xie et al., 2015). Surpris- 2002). In conclusion, the optimized heterostructure of InAs/
ingly, IR detector technologies operate specifically at cryogenic InGaAs/GaAs QDIPs have exhibited high responsivity of 700 mA/W,
temperatures and variation in the temperature would alter the it was mainly attributed to the enlarged IR absorption under
detection range of the device. For burgeoning the infrared detector increased QD layers.
technology, quantum well-infrared photodetectors (QWIPs) used Similarly, Al0.3Ga0.7As/GaAs heterostructure including InAs
for MWIR detection, which commercially well established in the quantum-dot (QD) layer with a 10 nm thick GaAs spacer was
current market (Levine et al., 1992; Gunapala et al., 1991; W. Tang developed as a mid-infrared sensor (Murata et al., 2020). The
et al., 2018; Rodriguez et al., 2018; Wu et al., 2018). It is inter- photodetector developed on nþ-GaAs (001) substrate using mo-
esting to highlight that quantum dot infrared photodetectors lecular beam epitaxy (MBE) technique. Later, intrinsic GaAs layer
(QDIPs) used for LWIR and VLWIR detection (Ramiro et al., 2020; (300 nm), InAs QDs, GaAs capping layer (10 nm), and Al0.3Ga0.7As
Chen et al., 2020c). Specifically, QDIPs are commendable to over- layer (20 nm) were sequentially developed. Au and AueGe elec-
come the QWIPs technology towards MWIR detection. Currently, trodes were used to achieve the ohmic-contact behaviour between
various research groups involved in developing the promising the electrode and photo-active material. As a result, Al0.3Ga0.7As/
quantum dot technology for strengthening the optical properties GaAs composite exhibited the responsivity of 0.8 A/W at 295 K and
due to the fact that electrons are confined in 3-D space (Keuleyan specific detectivity of 1.8  1010 Jones under 6.6 mm IR wavelength
et al., 2011). Remarkably, QDIPs possess superior properties illumination. The accumulated electrons at the interface of heter-
compared to QWIPs such as outstanding charge carrier lifetime ostructure transferred to the conduction band of Al0.3Ga0.7As bar-
(10e100 times), grating free usage, and more stable during tem- rier by means of two factors. The first one can be illumination of IR
perature fluctuations. In this section, we mainly focused on the light and other factor was drift produced by the electric field at the
junction. Fig. 10(a) presents the energy states for limited charge

14
P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Fig. 10. (a) The proposed energy states for limited carriers at the hetero-interface of TPU-SC with InAs QDs (Asahi et al., 2017) and (b) Graphic illustration of InAs QD avalanche
photodiodes deposited on GoVS substrate (Chen et al., 2020a).

carriers at the hetero-interface of two-step photon up-conversion- vapor deposition technique (MOCVD). APD epitaxial structure was
solar cell (TPU-SC) with InAs QDs (Asahi et al., 2017). The presence developed using molecular beam epitaxy (MBE). After deposition,
of InAs QDs significantly induces the intraband transitions, which the epitaxial structure was etched into a wave guide shape by
was mainly due to the electronic wave functions spatially quantized inductive coupled plasma. Then the sidewalls of wave guide were
by the QDs irrespective of the incident light polarization (Tas et al., passivated with Al2O3 layer to arrest the leakage current. In such a
2012). way, Pd/Ti/Pd/Au and Pd/Ge/Pd/Au were used as metal stack con-
Very recently, avalanche photodiode (APD) based InAs quantum tacts. Fig. 10(b) presents the overall layer-by-layer device archi-
dot IR photodetectors were studied under low dark current gen- tecture of InAs QD avalanche photodiodes deposited on GoVS
eration (Chen et al., 2020b) The QD-APD was deposited on GaAs- substrate. Here, InAs quantum dot waveguide APD was mono-
on-V-grooved-Si (GoVS) substrate by metal-organic chemical lithically deposited onto the Si substrate. Accordingly, the

Fig. 11. (a) Graphic diagram of graphene transistor tailored with PbS QDs, (b) responsivity of PbS QD/graphene heterojunction under the IR illumination with different IR intensities,
and (c) band diagram along with charge generation at a PbS QD/graphene heterojunction under the IR illumination (Sun et al., 2012).

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

fabricated device exhibited the lower dark current (0.1 nA) with used as top layer to absorb the UV and visible spectra. The detection
responsivity of 0.234 A/W. range was able to tune from 800 nm to the onset absorption
wavelength of the bottom-QD layer through the OTP/QD ss-PDs.
4.2. Pb, Ge and Hg based quantum dot infrared photodetectors Further, depending on the size of the QDs, we can achieve the
essential IR detection range. Based on the above constructive fea-
In addition to the above InAs QDs community, PbS QDs also tures, QD ss-PDs achieved superior responsivity (15.6 mA/W) and
streamlined to achieve superior IR photodetection. Building upon detectivity (1.3  1011 Jones) under IR light (930 nm). Therefore,
this knowledge on PbS QDs, graphene integrated PbS QDs identified introduction of OTP as a top layer can highly beneficial for removal
as efficient IR photodetector (Sun et al., 2012). To prove viability of of non-target spectrum, which is energetically favorable for selec-
PbS QDs, graphene sheets were synthesized on the copper sub- tive IR detection.
strate by conventional CVD technique. Later, graphene sheets were Another type of PbS QD based composite favorable for the IR
transferred onto the Si substrate. Finally, PbS QDs developed onto photodetector performance. Interestingly, graphene-PbS QD com-
the graphene using facile solution processing technique. Fig. 11 (a) posite provided unique opportunity to study the near-infrared
presents the graphene modified PbS QDIP device structure. In this photodetector performance (Jeong et al., 2020). Initially, single-
creative study, IR responsivity of PbS QDs based device significantly layer graphene flakes and PbS QDs capped with oleic acid were
increased with decrease of light intensity (32.7 mW/ separately synthesized. Later, the solution was mixed using con-
cm2 < 12.3 mW/cm2 < 221 nW/cm2 < 14.5 nW/cm2). They found ventional sonication process in hexane solution. Finally, the
that PbS QDIP device is capable of superior responsivity of 1  107A/ graphene-PbS QDs mixture was coated onto a glass substrate. The
W at a selective low IR light (895 nm) intensity of 14.5 nW/cm2 as interdigitated finger patterns of Au electrodes were patterned onto
shown in Fig. 11 (b). On the other hand, the PbS QDIP device was the SiO2 substrate using the photolithography. Due to the
also developed on the flexible plastic substrate, which provided constructive interaction between graphene and PbS QDs,
excellent channel for the development of flexible photodetector. graphene-PbS QDs composite exhibited higher photocurrent (5
Considering the interaction between PbS-QDs and graphene sheets, times), 22% of less rise time and 47% of shorter decay time
it is plausible to expect the high detection capability, which re- compared to the pure PbS QDs. Overall, the impressive enhance-
mains an attractive feature for superior charge transportation from ment in the photodetector performance mainly ascribed to the
PbS-QDs to graphene (with high mobility). The corresponding en- photo-induced charge transportation in the graphene-PbS QD
ergy levels alignment between graphene and PbS-QD, charge car- composite.
rier generation and separation under IR illumination presented in Recently, the concept of large-scale production of spray depos-
the Fig. 11(c). ited PbS QDs addressed for IR photodetector (Chen et al., 2020c).
In another study, high-speed PbSe QD photodetector was This approach also compared with the QD-solids prepared by the
fabricated using sandwich micro-strip transmission line structure simple spin-coating technique. The spray deposition technique al-
(Gao et al., 2016). Here, solution processed PbSe-QD films sand- lows the QDs to establish the dense packing. Fig. 12(a) presents the
wiched between ITO electrode (bottom) and gold electrode (top). PbS QDs photodetector device structure. Due to the dense packing,
This device architecture was particularly noticeable for ultra-high- charge carrier density can be improved, and band gap can be nar-
speed IR photodetector performance with EQE of ~50%, respon- rowed among the neighboring QDs. Taking into the account, IR
sivity of 0.36 A/W, and response time of 74 ps at room temperature photodetector performance can be significantly increased.
under carrier sweep mechanism. Such a striking IR photodetector Fig. 12(b) presents the IR photodetector performance of spray and
performance realized by the tiny overlapping area of 100 mm2 spin coated PbS QDs. The spray deposited samples determine the
electrodes. higher photon currents compared to the spin coated PbS QDs over
Although limited research focused on spectral selective photo- range IR wavelengths (800e1400 nm) with intensity of 430 mW/
detection, the unique structure of PdS QDs ground for the spectral cm2. As a result, spray deposited PbS QDIPs exhibited superior
selective IR photodetector performance (ss-Pds) (Qiao et al., 2016). responsivity (365.1 A/W) and detectivity (1.4  1012 Jones) under IR
In this work, they reported the absorption characteristics (at light of wavelength 1250 nm with intensity of 63.5 mW/cm2. Finally,
wavelengths of 800 nm, 880 nm, 1140 nm, and 1480 nm) powered this study considers the importance of spray deposition technique
by the QD size effect. The organolead triiodide perovskite (OTP) was for developing the potential large-scale IR photodetectors.

Fig. 12. (a) PbS quantum dots photodetector device and (b) photon current behavior of spin and spray coated PbS quantum dots photodetector (Chen et al., 2020c).

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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

Table 3
Comparison of IR photodetector performance with different nanostructured materials.

Materials Methodology Photocurrent (mA) Responsivity (A/W) Detectivity (Jones) EQE (%) Ref

InAs QDs MBE e 0.7 33  1011 e Kim et al. (2004)

Al0.3Ga0.7As/GaAs/InAs QDs MBE 20 0.8 1.8  1010 e Murata et al. (2020)
InAs QD APD MOCVD e 0.234 e e Chen et al. (2020a)
PbS-QDs/graphene CVD 6  103 1  107 e e Sun et al. (2012)
PbSe QDs Dip coating e 0.36 e 50 Gao et al. (2016)
Ss PbS QDs Spin coating 15.6  103 1.3  1011 e Qiao et al. (2016)
Graphene-PbS QD Sonication 5.4  103 e e e Jeong et al. (2020)
PbS QD Spray deposition e 365.1 1.4  1012 e (Chen et al., 2020c)
SWCNT-PbS QD Spin coating 31.1 7.2 7.1  1010 e Tang et al. (2018)
GeQD/SiNW PECVD 22  103 1.5  103 e e Zhao et al. (2020)
HgSe/HgTe NC Spin coating 10  103 ~1  103 1.5  109 e Livache et al. (2019)
GNR Drop casting 2725 1 e e Chitara et al. (2011)

Further, adaptive single-walled carbon nanotubes (SWCNTs) to improve the IR photodetector performance of graphene, which
combined with PbS QDs (SWCNT-PbSQD), which directed to ach- can be solved by developing multilayer stacking on Si substrate. As
ieve IR photodetector performance (Y. Tang et al., 2018). For a result, multilayer stacking can scale up the IR absorption capacity
SWCNT-PbSQD, SWCNTs were deposited on the Si/SiO2 substrate up to ~25%, which is comparatively higher than bi-layer (4.6%) and
using the dip-coating method. The interdigited electrode pattern tri-layer (6.9%) of graphene under normal incident of IR light at
was designed using electron beam lithography. Later, this pattern 1550 nm wavelength.
allows to develop the Pd (3 nm) and Au (50 nm) electrodes using In conclusion, we have systematically discussed the viability of
thermal evaporation technique. Finally, PbS QD solution was InAs and PbS based QDs towards efficient IR photodetector per-
adapted as layer by layer using spin coating on SWCNTs. As a result, formance. In an attempt to address the IR photodetector perfor-
the developed SWCNT-PbSQD architecture underlined the mance based on InAs ODs, Al0.3Ga0.7As/GaAs hetero-structure
responsivity of 7.2 A/W, specific detectivity of 7.1  1010 Jones, and consisting of InAs QDs exhibited outstanding IR responsivity (0.8
response time of 1.58 ms at IR wavelength of 1550 nm (141.47 mW/ A/W) at 6.6 mm wavelength compared to the other InAs QD pho-
cm2). At the most fundamental level, internal electric field todetectors. Moreover, QDIPs based PbS QDs have shown improved
approximated the light-induced charge carrier separation at the IR photodetector performance compared to the InAs-based pho-
interface of SWCNT and PbSQDs. Overall, SWCNT-PbSQD combi- todetectors. In such a way, PbS-QDs/graphene composite achieved
nation is essential for superior IR photoresponse and detectivity. remarkable responsivity (107 A/W) under IR irradiation, which
In a similar vein, germanium quantum dot (GeQDs) infrared attributed to the superior charge carrier transportation at the
photodetectors were developed at low temperature (<300  C) interface under ultrahigh mobility of graphene. Also, the possibility
(Zhao et al., 2020). In this method, the SieGe bilayer was converted of deposition technique (spray deposition) makes the PbS QDs
into Si/Ge heterostructured nanowires by rolling of indium (In) more responsive to encourage the IR light (365 A/W) and detec-
droplets at 300  C. Later, Indium droplets absorbed into the bilayer tivity (1.4  1012 Jones) under controlled higher density of PbS QDs.
precursor and self-modulated to produce GeQDs. Interestingly, On the other hand, HgSe/HgTe nanostructures presented poor
SiNWs as a metal electrode demonstrated the possibility of supe- responsivity due to absorption layer of HgSe/HgTe nanocrystals was
rior IR absorption. As a result, the developed samples have shown very thin. The mechanism of generating photocurrent in QDIPs is
the IR responsivity about 1.5 mA/W (at l ¼ 1550 nm). It demon- due to intraband excitation of electrons upon illumination with
strates the possibility to integrate the individual GeQDs into Si photons. The photo-excitation of electrons takes place from
complementary metal oxide semiconductor (CMOS) circuits to- confined states of conduction band dots to the continuum.
wards IR detection, high-density IR communication, and imaging. Improved QDIPs performance could be due to lower dark current
Colloidal nanocrystals also extensively used, since they have the attributed to the 3-D confinement of electron wave function,
ability to achieve the broad spectral tunability (Livache et al., 2019). reduction in thermal generation of electrons due to quantization of
reported that energy landscape of quantum well and quantum dot energy in all three dimensions, and ability to inter-sub-band ab-
IR photodetectors aped from combination of mercury selenide sorption even at normal incidence. The comprehensive IR photo-
(HgSe) and mercury telluride (HgTe) nanocrystals. This strategic detection performance of various QDs is tabulated in Table 3.
metamaterial combination provides intraband absorption under
superior transport properties such as fast time response, low dark
5. Conclusions and future perspectives
current, and large thermal activation energy. In such a way, the
responsivity and detectivity values were found to be ~5 mA/W and
In this review, we have systematically summarized the recent
1.5  109 Jones, respectively at 80 K. The obtained results were very
advancements in UV, visible, and IR photodetectors based on
less compared to the QDIPs (Deng et al., 2014). The reason behind
various adaptive heterostructures. Specifically, we categorized the
the less responsivity is lack of absorption through the very thin
novel functional materials such as (i) metal oxide thin films for UV
layer of NCs.
light detection, (ii) 1-D nanomaterials (NWs), 2-D nanosheets and
While the usage of ultrahigh mobility graphene exhibits
perovskite materials for visible light detection and (iii) 0-D (QDs,
promising visible light photodetector performance, it is limited in
NCs) for IR detection. Also, we emphasized the various device ar-
the IR region about 2% and resulting low responsivities. To study
chitectures, which significantly influenced the overall photode-
the capability of IR photodetector performance, rGO combined
tector performance.
graphene nanoribbons (GNR) were developed on SiO2/Si substrate
In depth, metal-oxide semiconductors (ZnO, Ga2O3, SnO2, TiO2,
using drop casting method (Chitara et al., 2011). Here, two elec-
and WO3) were given priority for UV light detection owning to their
trodes (Cr/Au) were coated in between rGO/GNR, which can give
suitable wide bandgap. For visible light photodetectors, we have
rise to the IR responsivity of 1 A/W. Thus, there are many challenges
systematically explored the graphene-based materials with
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P.V.K. Yadav, B. Ajitha, Y.A. Kumar Reddy et al. Chemosphere 279 (2021) 130473

different heterostructures (PQD/rGO, GaN/SLG, rGO/WSe2 and Declaration of competing interest

GeSn/graphene) and nanostructures (HgSe/HgTe NCs and WO3
NWs) owning to their broad band spectral absorption and ultra- The authors declare that they have no known competing
high mobility of graphene. However, due to the low absorption financial interests or personal relationships that could have
rate of pure graphene, graphene-based composites (rGO-CZS, PQD- appeared to influence the work reported in this paper.
rGO, N-SLG, and GO doped PbI2) dedicated to improve the photo-
response and EQE of resultant photodetector. It is to be noted that Acknowledgements
photogenerated charge carriers effectively separated at the heter-
ostructure interface to enhance the responsivity and detectivity. One of the author (Dr. Y. Ashok Kumar Reddy) would like to
Further, by synthesizing the nanostructures with high surface-to- express his gratitude to the Department of Science and Technology
volume ratio, the bandgap values were effectively tuned (WSe2 (DST), New Delhi, India for the award of DST-Inspire Faculty (DST/
and WO3), which was highly beneficial for visible light absorption INSPIRE//04/2017/002531).
and good responsivity. For IR photodetectors, mostly QD-based
materials (InAs QDs and PbS QDs) have been successfully utilized.
References
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